Initial Excitation Energy Research Articles

Modeling Photodissociation: Quantum Dynamics Simulations of Methanol.

A comprehensive computational study of the gas-phase photodissociation dynamics of methanol is presented. Using a multiconfigurational active space based method (RASSCF) to obtain multidimensional potential energy surfaces (PESs) on-the-fly, direct quantum dynamics simulations were run using the variational multi-configurational Gaussian method (DD-vMCG). Different initial excitation energies were simulated to investigate the dependence of the branching ratios on the electronic state being populated. A detailed mechanistic explanation is provided for the observed differences with respect to the excitation energy. Population of the lowest lying excited state of methanol leads to rapid hydroxyl hydrogen loss as the main dissociation channel. This is rationalized by the strongly dissociative nature of the PES cut along the O-H stretching coordinate, confirmed by the broad feature in the absorption spectrum. In contrast, more energetic excitations lead mainly to C-O bond breaking. Again, analysis of the diabatic surfaces offers a clear explanation in terms of the nature of the electronic states involved and the coupling between them. The type of calculations presented, as well as the subsequent analysis of the results, should be seen as a general workflow for the modeling of photochemical reactions.

Computational study of the adamantane cation: simulations of spectroscopy, fragmentation dynamics, and internal conversion

Diamondoids, of which adamantane (C_{10}H_{16}) is the simplest representative, constitute an intriguing class of carbon based nanomaterials with interesting chemical, mechanical and opto-electronic properties. While neutral diamondoids have been extensively studied for decades, their cationic counterparts were a subject of recent experimental investigations motivated by their potential role in astrochemistry. Here, we perform a computational study of the adamantane cation (C_{10}H_{16}^+) complementing the recent experimental findings. Specifically, we extend earlier theoretical work on vibrationally resolved electronic spectroscopy by accounting for the higher lying electronically excited states of the cation in the absorption and photoelectron spectra. We also perform adiabatic and nonadiabatic (surface hopping) molecular dynamics simulations to study (fast) fragmentation processes and electronic relaxation of C_{10}H_{16}^+. Our simulations reveal that after excitation with near-infrared–ultraviolet photons, the adamantane cation undergoes an ultrafast internal conversion to the ground (doublet) state (on a time scale of 10–100 fs depending on initial excitation energy) which can be followed by a fast fragmentation, predominantly H loss. The yield of the ultrafast hydrogen dissociation as a function of excitation energy is reported.

Propagation of supersonic soliton in carbon nanotubes of armchair type

The propagation of a localized ring nonlinear wave in carbon nanotubes (CNTs) of armchair type has been explored using the MD/DFTB method. It is unambiguously shown that the considered localized waves are soliton-type. Herewith, the higher a velocity of an initial perturbation, the higher a steady-state velocity of the considered soliton. It is established that at a high initial excitation energy in a time period of 0.1-0.2 ps the soliton moves at the speed in the range of 245-270 Angstrem/ps, which is approximately in 1.22-1.35 times higher than the speed of sound in CNTs (200 Angstrem/ps). It is shown that the soliton velocity practically does not change with increasing CNT radius Keywords: molecular dynamics, carbon nanotubes, soliton, supersonic wave.

Распространение сверхзвукового солитона в углеродных нанотрубках типа кресло

The propagation of a localized ring nonlinear wave in carbon nanotubes (CNTs) of armchair type has been explored using the MD/DFTB method. It is unambiguously shown that the considered localized waves are soliton-type. Herewith, the higher a velocity of an initial perturbation, the higher a steady-state velocity of the considered soliton. It is established that at a high initial excitation energy in a time period of 0.1-0.2 ps the soliton moves at the speed in the range of 245-270 Å/ps, which is approximately in 1.22-1.35 times higher than the speed of sound in CNTs (200 Å/ps). It is shown that the soliton velocity practically does not change with increasing CNT radius

Nuclear level densities and γ -ray strength functions in Sn120,124 isotopes: Impact of Porter-Thomas fluctuations

Nuclear level densities (NLDs) and $\gamma$-ray strength functions (GSFs) of $^{120,124}$Sn have been extracted with the Oslo method from proton-$\gamma$ coincidences in the ($p,p^{\prime}\gamma)$ reaction. The functional forms of the GSFs and NLDs have been further constrained with the Shape method by studying primary $\gamma$-transitions to the ground and first excited states.The NLDs demonstrate good agreement with the NLDs of $^{116,118,122}$Sn isotopes measured previously. Moreover, the extracted partial NLD of 1$^{-}$ levels in $^{124}$Sn is shown to be in fair agreement with those deduced from spectra of relativistic Coulomb excitation in forward-angle inelastic proton scattering. The experimental NLDs have been applied to estimate the magnitude of the Porter-Thomas (PT) fluctuations. Within the PT fluctuations, we conclude that the GSFs for both isotopes can be considered to be independent of initial and final excitation energies, in accordance with the generalized Brink-Axel hypothesis. Particularly large fluctuations observed in the Shape-method GSFs present a considerable contribution to the uncertainty of the method, and may be one of the reasons for deviations from the Oslo-method strength at low $\gamma$-ray energies and low values of the NLD (below $\approx1\cdot10^{3}-2\cdot10^{3}$ MeV$^{-1}$).

Discrete breathers and energy localization in a nonlinear honeycomb lattice.

Discrete breathers (DBs) in nonlinear lattices have attracted much attention in the past decades. In this work, we focus on the formation of DBs and their induced energy localization in the nonlinear honeycomb lattice derived from graphene. The key step is to construct a reduced system (RS) with only a few degrees of freedom, which contains one central site and its three nearest neighbors. The fixed points and periodic orbits of the RS can be obtained from the Poincaré section of the dynamics. Our main finding is that the long-running DB solution of the full honeycomb system corresponds to the periodic orbit given by one of the fixed points of RS, where the central site and its nearest neighbors vibrate inversely. When the initial condition deviates from this fixed point, the local vibration is attracted to it after a short transient process. When the initial condition is assigned to other fixed points of the RS, the initial excitation energy flows to the other part of the full system quickly, resulting in a delocalized wave propagation. Another main finding is that the long-lived DB solutions emerge only when the initial excitation energy is larger than a threshold value, above which the frequency of the DB exceeds the phonon band edge. The excitation energy generally dissipates from the local region due to the interactions between the DB and phonons near the Γ point in the dispersion relation. These results provide a holistic physical picture for the DB solutions in two-dimensional nonlinear lattices with complex potentials, which will be crucial to the understanding of energy localization in the realistic two-dimensional materials.

Energy and pairing dependence of dissipation in real-time fission dynamics

This work presents a microscopic study of dissipation in fission dynamical evolutions with the time-dependent Hartree-Fock+BCS method in terms of energy dependence and pairing dependence. The friction coefficients and dissipation energies are extracted by mapping the symmetric fission process of $^{258}$Fm into a classical equation of motion. Density-constrained calculations are used to obtain the dynamical potential. The obtained friction coefficients have a strong dependence of deformations, and averagely match the coefficients adopted in statistical models. The dissipation indeed increase with increasing initial excitation energies or with decreasing pairings. It is also shown that post-scission dissipations play a significant role. The demonstrated characteristics of dissipations will be valuable for calibrations of various fission models.

Deformation Parameters and Collective Temperature Changes in Photofission Mass Yields of Actinides Within the Systematic Statistical Scission Point Model

The photofission fragment mass yields of actinides are evaluated using a systematic statistical scission point model. In this model, all energies at the scission point are presented as a linear function of the mass numbers of fission fragments. The mass yields are calculated with a new approximated relative probability for each complementary fragment. The agreement with the experimental data is quite good, especially with a collective temperature Tcol of 2 MeV at intermediate excitation energy and Tcol = 1 MeV for spontaneous fission. This indicates that the collective temperature is greater than the value obtained by the initial excitation energy. The generalized superfluid model is applied for calculating the fragment temperature. The deformation parameters of fission fragments have been obtained by fitting the calculated results with the experimental values. This indicates that the deformation parameters decrease with increasing excitation energy. Also, these parameters decrease for fissioning systems with odd mass numbers.

Energy sharing based on microscopic level densities

The transformation of a moderately excited heavy nucleus into two excited fission fragments is modeled as a strongly damped evolution of the nuclear shape. The resulting Brownian motion in the multi-dimensional deformation space is guided by the shape-dependent level density which has been calculated microscopically for each of nearly ten million shapes (given in the three-quadratic-surfaces parametrization) by using a previously developed combinatorial method that employs the same single-particle levels as those used for the calculation of the pairing and shell contributions to the five-dimensional macroscopic-microscopic potential-energy surface. The stochastic shape evolution is followed until a small critical neck radius is reached, at which point the mass, charge, and shape of the two proto-fragments are extracted. The available excitation energy is divided statistically on the basis of the microscopic level densities associated with the two distorted fragments. Specific fragment structure features may cause the distribution of the energy disvision to deviate significantly from expectations based on a Fermi-gas level density. After their formation at scission, the initially distorted fragments are being accelerated by their mutual Coulomb repulsion as their shapes relax to their equilibrium forms. The associated distortion energy is converted to additional excitation energy in the fully accelerated fragments. These subsequently undergo sequential neutron evaporation which is calculated using again the appropriate microscopic level densities. The resulting dependence of the mean neutron multiplicity on the fragment mass, as well as the dependence of on the initial excitation energy of the fissioning compound nucleus, exhibit features that are similar to the experimentally observed behavior, suggesting that the microscopic energy sharing mechanism plays an important role in low-energy fission.

Probing the Jacobi shape transition in hot and rotating Sc43

The evolution of the hot and rotating $^{43}\mathrm{Sc}$ nucleus to a highly deformed shape has been studied by measuring the high-energy $\ensuremath{\gamma}$ rays from the decay of the giant dipole resonance. The compound nucleus was populated at two initial excitation energies and average angular momenta of $\ensuremath{\approx}26$ and $31\ensuremath{\hbar}$ by using $^{16}\mathrm{O}$ beam of energies ${E}_{\mathrm{lab}}$ = 120 and 142 MeV, respectively. The evaporated neutron energy spectra have been measured for proper determination of nuclear level density. The angular momentum has been determined by measuring the low-energy $\ensuremath{\gamma}$-ray multiplicities. The high-energy $\ensuremath{\gamma}$-ray and neutron spectra were analyzed simultaneously. At $\ensuremath{\langle}J\ensuremath{\rangle}\ensuremath{\approx}26\ensuremath{\hbar}$ a near-oblate shape is observed, whereas at $\ensuremath{\langle}J\ensuremath{\rangle}\ensuremath{\approx}31\ensuremath{\hbar}$ a sharp peak is observed at ${E}_{\ensuremath{\gamma}}\ensuremath{\approx}10\phantom{\rule{0.28em}{0ex}}\mathrm{MeV}$ pointing towards the transition to the Jacobi shape with quadruple deformation parameter $\ensuremath{\beta}\ensuremath{\approx}0.7$. The results have been corroborated by the theoretical calculations based on the rotating liquid drop model framework.

Fragmentation Patterns of Radiosensitizers Metronidazole and Nimorazole upon Valence Ionization.

We study gas-phase photodissociation of radiosensitizer molecules nimorazole and metronidazole with the focus on the yield of the oxygen mimics nitrogen oxides and nitrous acid. Regardless of photon energy, we find the nimorazole cation to split the intramolecular bridge with little NO2 or NO production, which makes the molecule a precursor of dehydrogenated methylnitroimidazole. Metronidazole cation, on the contrary, has numerous fragmentation pathways with strong energy dependence. Most notably, ejection of NOOH and NO2 takes place within 4 eV from the valence ionization energy. Whereas the NO2 ejection is followed by further fragmentation steps when energy so allows, we find emission of NOOH takes place in microsecond time-scales and as a slow process that is relevant only when no other competing reaction is feasible. These primary dissociation characteristics of the molecules are understood by applying the long-known principle of rapid internal conversion of the initial electronic excitation energy and by studying the energy minima and the saddle points on the potential energy surface of the electronic ground state of the molecular cation.

Crossover from weak to strong quench in a spinor Bose-Einstein condensate

We investigate the early-time dynamics of a quasi-two-dimensional spin-1 antiferromagnetic Bose-Einstein condensate after a sudden quench from the easy-plane to the easy-axis polar phase. The post-quench dynamics shows a crossover behavior as the quench strength $\tilde{q}$ is increased, where $\tilde{q}$ is defined as the ratio of the initial excitation energy per particle to the characteristic spin interaction energy. For a weak quench of $\tilde{q}<1$, long-wavelength spin excitations are dominantly generated, leading to the formation of irregular spin domains. With increasing $\tilde{q}$, the length scale of the initial spin excitations decreases, and we demonstrate that the long-wavelength instability is strongly suppressed for high $\tilde{q}>2$. The observed crossover behavior is found to be consistent with the Bogoliubov description of the dynamic instability of the initial spinor condensate.

Excitation energy partition in fission

The transformation of an atomic nucleus into two excited fission fragments is modeled as a strongly damped evolution of the nuclear shape. As in previous studies, it is assumed that the division of mass and charge is frozen in at a critical neck radius of c0=2.5fm. In order to also determine the energetics, we follow the system further until scission occurs at a smaller neck radius, at which point the shapes of the proto-fragments are extracted. The statistical energy available at scission is then divided on the basis of the respective microscopic level densities. This approach takes account of important (and energy-dependent) finite-size effects. After the fragments have been fully accelerated and their shapes have relaxed to their equilibrium forms, they undergo sequential neutron evaporation. The dependence of the resulting mean neutron multiplicity on the fragment mass, ν¯(A), including the dependence on the initial excitation energy of the fissioning compound nucleus, agrees reasonably well with observations, as demonstrated here for 235U(n,f), and the sawtooth appearance of ν¯(A) can be understood from shell-structure effects in the level densities.

Controlled short time large scale synthesis of magnetic cobalt nanoparticles on carbon nanotubes by flash annealing

Nanopatterned arrays of discrete cobalt nanostructures showing characteristic parameter-dependent sizes are formed from continuous thin films on a carbon nanotube substrate using millisecond pulsed intense UV light. The nanoparticles exhibit ferromagnetic behavior with magnetic remanence and coercivity depending on the particle size. The end-state particle size is shown to be a function of initial thin film thickness and excitation energy and is therefore tunable. The evolutionary process from continuous thin films to a discrete morphology is thermodynamically driven by the large surface energy difference between metastable thin films and the underlying carbon nanotube substrate. Evidence of the Danielson model of the dewetting process is observed. These arrays can find applications as platforms for the self-assembly of magnetically susceptible materials, such as iron or nickel nanostructures, into a conduction matrix for applications in energy extraction from a latent heat storage device.

Insight into the Fission Process from Surrogate Reactions in Inverse Kinematics

Innovative experiments are conducted to widen our approach to fission, aiming notably at a complete identification and characterization of the fragments and the study of unstable fissioning systems. In the GANIL facility, full fission-fragment distributions and fragment kinetic energies are measured, thanks to the inverse kinematics technique and the magnetic spectrometer VAMOS. The access to the scission-point information is possible thanks to the low-energy regime. The initial excitation energy of the systems is also determined due to the well-defined transfer reactions. In this work, fission yields and fission-fragment kinetic energies of 239U, as well as the evolution of the yields with the initial excitation energy of 240Pu, are presented.

Sequential binary decay of highly excited 40Ar*

The sequential statistical binary decay of the highly excited compound nucleus 40Ar* is described with an extended evaporation formalism implemented in a Monte-Carlo multi-step statistical model code. Asymmetric mass splittings involving nucleon emission up to symmetric binary ones are treated within the evaporation formalism, in a unified manner. Emission of heavy fragments in their ground and excited (particle-bound or unbound) states is considered. The evolution of the final mass distributions from 40Ar* is studied as a function of the initial excitation energy, in the range from 45 up to 405 MeV. The population of final states originating from the decay of intermediate mass fragments in particle-bound and particle-unbound states (side-feeding) is discussed. Results are compared with an alternative description in which the time-dependent decay process is described by rate equations for the generation of different fragment species.

Fission dynamics of Pu240 from saddle to scission and beyond

Calculations are presented for the time evolution of $^{240}\mathrm{Pu}$ from the proximity of the outer saddle point until the fission fragments are well separated, using the time-dependent density functional theory extended to superfluid systems. We have tested three families of nuclear energy density functionals and found that all functionals exhibit a similar dynamics: The collective motion is highly dissipative and with little trace of inertial dynamics, due to the one-body dissipation mechanism alone. This finding justifies the validity of using the overdamped collective motion approach and to some extent the main assumptions in statistical models of fission. This conclusion is robust with respect to the nuclear energy density functional used. The configurations and interactions left out of the present theory framework only increase the role of the dissipative couplings. An unexpected finding is varying the pairing strength within a quite large range has only minor effects on the dynamics. We find notable differences in the excitation energy sharing between the fission fragments in the cases of spontaneous and induced fission. With increasing initial excitation energy of the fissioning nucleus, more excitation energy is deposited in the heavy fragment, in agreement with experimental data on average neutron multiplicities.

Fusion-fission dynamics of Pt188,190 through fission fragment mass distribution measurements

Fission fragment mass distributions have been measured for relatively neutron-deficient compound nuclei, $^{188}\mathrm{Pt}$ and $^{190}\mathrm{Pt}$, formed in the fusion reactions, $^{28}\mathrm{Si}+^{160}\mathrm{Gd}$ and $^{12}\mathrm{C}+^{178}\mathrm{Hf}$, respectively. The data were obtained for a similar initial excitation energy range of 49--68 MeV for both the systems. The fragment mass distributions for both the Pt isotopes were found to be single peaked and no appreciable change in the mass symmetry was observed throughout the measured excitation energy range, for both the reactions. However, relatively broader mass distributions observed in the fission of $^{188}\mathrm{Pt}$ in the studied energy domain indicates the presence of fission events originating from a nonequilibrated source as well. This signifies that the mass equilibrium has not been fully achieved in the $^{28}\mathrm{Si}+^{160}\mathrm{Gd}$ system as compared to the $^{12}\mathrm{C}+^{178}\mathrm{Hf}$ system, indicating the presence of quasifission events in the former reaction.

Using excitation-energy dependent fission yields to identify key fissioning nuclei in r-process nucleosynthesis

The possibility that nucleosynthesis in neutron star mergers may reach fissioning nuclei introduces significant uncertainties in predicting the relative abundances of r-process material from such events. We evaluate the impact of using sets of fission yields given by the 2016 GEF code for spontaneous (sf), neutron-induced ((n, f)), and β-delayed (βdf) fission processes which take into account the approximate initial excitation energy of the fissioning compound nucleus. We further explore energy-dependent fission dynamics in the r process by considering the sensitivity of our results to the treatment of the energy sharing and de-excitation of the fission fragments using the FREYA code. We show that the asymmetric-to-symmetric yield trends predicted by GEF 2016 can reproduce the high-mass edge of the second r-process peak seen in solar data and examine the sensitivity of this result to the mass model and astrophysical conditions applied. We consider the effect of fission yields and barrier heights on the nuclear heating rates used to predict kilonova light curves. We find that fission barriers influence the contribution of 254Cf spontaneous fission to the heating at ∼100 d, such that a light curve observation consistent with such late-time heating would both confirm that actinides were produced in the event and imply the fission barriers are relatively high along the 254Cf β-feeding path. We lastly determine the key nuclei responsible for setting the r-process abundance pattern by averaging over thirty trajectories from a 1.2–1.4 M⊙ neutron star merger simulation. We show it is largely the odd-N nuclei undergoing (Z, N)(n, f) and (Z, N)βdf that control the relative abundances near the second peak. We find the ‘hot spots’ for β-delayed and neutron-induced fission given all mass models considered and show most of these nuclei lie between the predicted N = 184 shell closure and the location of currently available experimental decay data.

Pre-saddle and pre-scission neutron emission rates in heavy-ion induced fission of 16O +208Pb and 16O +209Bi systems

Whereas there is a slight information on the pre-saddle neutron emission rate and neutron multiplicity, as well as it is impossible to separate the pre-saddle and saddle to scission neutron contributions experimentally, the theoretical studies of pre-saddle neutron emission rate and neutron multiplicity are of great importance. In the present work, the calculations of pre-saddle neutron multiplicity are performed using the analysis of fission fragment angular anisotropy data for [Formula: see text] and [Formula: see text] reaction systems. The obtained results show that the pre-saddle neutron multiplicity decreases by increasing the initial excitation energy and it has found to be characterized by a nonlinear behavior. Through the analysis of pre-saddle neutron multiplicity and pre-saddle transition time by means of the neutron clock method, the pre-saddle neutron emission rate is calculated for the first time. The findings of this study show that the pre-scission neutron emission rate is lower than the pre-saddle neutron emission rate.